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Physical Review A

Classical theory ofl-changing transitions in collisions between Rydberg atoms and ions

Andrey K. Kazansky, Valentin N. Ostrovsky

Published Sep 1, 1995• 15 citations
Publisher

Abstract

The l-changing transitions in collisions of Rydberg atoms with ions, A(${\mathit{nl}}_{0}$)+${\mathit{B}}^{+}$\ensuremath{\rightarrow}A(nl)+${\mathit{B}}^{+}$, are considered within the classical approximation for atomic electron motion. The elliptic orbit of the electron evolves slowly under the influence of the time-dependent electric field exerted by the incident ion. The quantum electron state is represented by an ensemble of classical trajectories. Within the dipole approximation extremely simple analytical formulas for the final-state l-distribution function are obtained for a fixed value of the impact parameter. The influence of the non-Coulomb core is taken into account approximately. The results of our calculations compare favorably with recent experimental data for the ${\mathrm{Na}}^{+}$(26d, 28d) Rydberg atom. The method can be extended to the calculation of distributions over various observables other than l.

DOI
10.1103/physreva.52.r1811

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The l-changing transitions in collisions of Rydberg atoms with ions, A(nl0{\mathit{nl}}_{0}nl0​)+B+{\mathit{B}}^{+}B+\ensuremath{\rightarrow}A(nl)+B+{\mathit{B}}^{+}B+, are considered within the classical approximation for atomic electron motion. The elliptic orbit of the electron evolves slowly under the influence of the time-dependent electric field exerted by the incident ion. The quantum electron state is represented by an ensemble of classical trajectories. Within the dipole approximation extremely simple analytical formulas for the final-state l-distribution function are obtained for a fixed value of the impact parameter. The influence of the non-Coulomb core is taken into account approximately. The results of our calculations compare favorably with recent experimental data for the Na+{\mathrm{Na}}^{+}Na+(26d, 28d) Rydberg atom. The method can be extended to the calculation of distributions over various observables other than l.
Transitions between states with the same principal quantum number n in the collision of a Rydberg atom with an ion are described within the classical approximation for the Rydberg electron. The quantum electron state is represented by an ensemble of classical trajectories. Within the dipole approximation for the interaction the final value of the orbital momentum l is calculated analytically for each initial trajectory in the ensemble. Averaging over the ensemble gives the distribution function over l. For the initial s state of the Rydberg atom the distribution functions are found also for the pairs of variables, namely: {the angular momentum; its projection on the collision velocity}; {projections of the angular momentum and the Runge - Lenz vector on the collision velocity} and {projections of the angular momentum and the Runge - Lenz vector on the plane perpendicular to the collision velocity}. The l-distributions for the orbitally polarized initial p and d Rydberg states with definite projections of the initial angular momentum on the velocity axis are also obtained. The influence of the non-Coulomb core is taken into account by an approximation. The final l-distributions (calculated for the initial s-state) are shifted towards the large-l values as the relative collision velocity vn decreases. Good agreement is achieved with the recent experimental data for Na(28d) and Na(26d) Rydberg atoms.
New experimental results have been obtained in collisions of singly charged ions with Na Rydberg atoms. (a) The distribution of final n states populated by electron capture shows non-monotonic variations of width with incident energy over the range 60-2100 eV. (b) The total capture cross section for alkali ions on Rydberg targets shows peaks and dips over the same energy range, correlated with particular reduced velocities v and the polarization of the exciting laser. (c) {ell}-Changing collision of Na{sup +} on Na(nd) targets, n=26 and 28, at low v preferentially transfer multiple units {h_bar} of orbital angular momentum under single-collision conditions, despite very large impact parameters. (d) Inelastic impacts of Na{sup f+} on Na 36s and 30p states, perturbed by electric fields, populate a strongly field-dependent mixture of nearby Stark levels. A synopsis of recent progress will be given.
A classical model for l mixing of Rydberg states in atomic collisions is described. The primary assumption of the model is that l changing occurs in a single hard-sphere collision between the Rydberg electron and the perturbing atom which is represented by the zero-energy scattering length L. Predictions of the model, which are in the form of cross sections as functions of principal quantum number n, are compared with data for l mixing of Na(nd) and Rb(nf) by rare-gas atoms. Agreement is, in most cases, quite good, comparable with that of other, more sophisticated, models. It is shown that, because the calculation must be carried out in the reference frame of the ion core, the energy deficit between low angular momentum states and the nearest hydrogenic manifold can be made up in a single collision between the Rydberg electron and the perturbing atom, an effect that is analogous to the gravitational slingshot effect used to alter the orbits of a spacecraft under the influence of the Sun's gravitational field. Comparison of data for l mixing by ground-state Rb atoms with model calculations in which L is treated as a free parameter leads to an estimate of 10 a.u. for the zero-energy scattering length of Rb.
A theory of inelastic n,l-changing and quasielastic l-mixing collisions of Rydberg atoms with the heavy rare-gas atoms is developed. It is based on the semiclassical impact-parameter approach combined with the normalized perturbation theory. Semiclassical formulas for scaled transition probabilities and cross sections as functions of the inelasticity parameter and the collision strength are analyzed. This approach gives a general description of collisional nl\ensuremath{\rightarrow}${\mathit{n}}^{\ensuremath{'}}$ transitions independently of the specific values of the principal quantum number, the relative velocity, and the type of colliding atoms. The energy and angular dependence of the electron-atom scattering amplitude is included in the theory by incorporating the impulse-approximation results in the weak-coupling limit. The Ramsauer-Townsend effect affects significantly the values of the cross sections, especially for the inelastic transitions with large energy transfer. The results obtained are used in calculations of the quenching cross sections for the Rb(nS,nD,nF) atoms in collisions with Ar, Kr, and Xe. Comparison of theory and experiment is made in a wide range of the principal quantum numbers and transition energy defects. \textcopyright{} 1996 The American Physical Society.
The theory of collisions of Rydberg atoms with rare-gas atoms is generalized to include the effects of an applied static electric field. Two effects occur. First, the field causes the states to split, and the increased energy separations lead to a decrease in the inelastic cross sections. Second, there is a change in the form of the wave functions, because the various Stark states in the field have electron charge distributions that may be localized in very different regions of space. The present work focuses on this second effect. With the description of the initial and final Stark states of the Rydberg atom by the proper electronic wave functions obtained in parabolic coordinates, cross sections are obtained for a variety of specific transitions of Rydberg atoms (n=10,15,and20n=10, 15, \mathrm{and} 20n=10,15,and20) caused by collisions. The calculations are strictly valid for hydrogen, but exhibit general features that are expected to apply to other Rydberg atoms as well. The results show a dramatic effect on the cross section for particular transitions depending on the degree of overlap of the initial and final charge distributions. In addition, it is observed that transitions are favored that involve small changes in the azimuthal quantum number mmm. The origin of this tendency is discussed.
The degree of dipole-forbidden l change in Na(26d) and Na(28d) Rydberg atoms caused by slow Na+{\mathrm{Na}}^{+}Na+ ion impact at reduced velocity v\ifmmode \tilde{}\else \~{}\fi{}=0.1--0.9 has been measured. Na+{\mathrm{Na}}^{+}Na+ beam energies 7.3--684 eV were used. Previous measurements were greatly improved by reducing stray electric fields in the Rydberg collision region to about 10 mV/cm. The distributions of final-angular-momentum states were analyzed using directly measured diabatic selective-field-ionization profiles for l=3, 4, and 5. l-change results in Na(26d) and Na(28d) targets are very similar and clearly show an increasing amount of dipole-forbidden behavior for decreasing reduced velocities v\ifmmode \tilde{}\else \~{}\fi{} and partial agreement with the coupled-channel calculation of Beigman and Syrkin (Zh. Eksp. Teor. Fiz. 89, 400 (1985) [Sov. Phys. JETP 62, 226 (1985)]). The dipole-forbidden process is the main channel for angular-momentum change in ion--Rydberg-atom collisions at v\ifmmode \tilde{}\else \~{}\fi{}\ensuremath{\le}0.7. At very low energy (v\ifmmode \tilde{}\else \~{}\fi{}\ensuremath{\le}0.3) the measurements demonstrate that the final-state distributions are dominated by very high angular-momentum states.